| Metal organic framework materials?MOFs?,as a highly versatile crystalline porous material with high specific surface area and a large number of active sites,have been widely used in gas storage and separation,drug transportation and catalysis.More importantly,the periodic network structure in the MOFs structure allows the spatial separation of unsaturated metal sites,which makes it better as a single-site catalyst for catalytic reactions.The abundant transition metal ions on the earth usually show good catalytic performance in chemical reactions.Based on the above reasons,the transition metal ions are linked with organic ligands to construct transition metal-based cobalt/nickel MOFs with metal active sites and applied to catalytic organic reactions,which has attracted wide attention.In this paper,several kinds of transition metal-based MOFs are introduced,and their structural characteristics and catalytic properties are studied.The full text is divided into four chapters:In the first chapter,we first introduce the metal-organic framework materials,and introduce the application of metal-organic framework materials in catalysis,and then introduce the application of metal-organic framework materials in the catalytic multi-component reaction.In chapter 2,two series of earth-abundant?M=Co,Ni?MOFs incorporating[M2??2-OH??COO?4]SBUs and linear carboxylate ligand were successfully synthesized by direct self–assembly methods with the formulae[?CH3?2NH2]-[M2??2-OH??COO?4?HDDIA??H2O?2]??solv?x?M-DDIA?,and[?CH3?2NH2][M2??2-OH??COO?4?TPTC??H2O?2]??solv?x??M-TPTC?[H5DDIA=2,5-di?3,5-dicarboxyl-phenyl?isonicotinic acid,H4TPTC=?1,1':4',1''-terphenyl?-3,3'',5,5''-tetracarboxy-lic acid].The two series of complexes exhibit a three-dimensional framework with nbo topology,and the two series of complexes contain highly dispersed coordination unsaturated metal sites and three nano cages evenly distributed,which may It is more conducive to capturing substrate molecules.At the same time,these complexes have high thermal stability and chemical stability,and the transition metal ions in the structure can be used as a potential Lewis acid site,making it a heterogeneous single-site Lewis acid catalyst with excellent catalytic activity.The solvent-free conditions exhibited excellent catalytic performance for the multicomponent Biginelli reaction.The third chapter mainly describes the method of using solvothermal,using the ligand 5,5',5''-?1,3,5-triazine-2,4,6-triamino?tristearate?H6TATAT?was synthesized with cobalt nitrate hexahydrate and nickel nitrate hexahydrate[?CH3?2NH2]6[Co?H2O?6]3{Co6??6-TATAT?4?H2O?12}?6H2O?Co-TATAT?and[?CH3?2NH2]6[Co?H2O?6]3{Ni6??6-TATAT?4?H2O?12}?6H2O?Ni-TATAT?,and for Co-TATAT and Ni-TATAT materials for The catalytic performance of the Biginelli reaction was studied under solvent conditions.The fourth chapter summarizes the single-site cobalt/nickel-MOFs and their multi-component reactions.This work provides a new basis for the construction of transition metal-based MOFs and their application in multi-component reactions. |
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